Electronic, Magnetic, and Theoretical Characterization of (NH4)4UF8, a Simple Molecular Uranium(IV) Fluoride
- 20 December 2018
- journal article
- research article
- Published by American Chemical Society (ACS) in Inorganic Chemistry
- Vol. 58 (1), 637-647
- https://doi.org/10.1021/acs.inorgchem.8b02800
Abstract
The simple system of tetraammonium octafluorouranate is employed to derive a fundamental understanding of the uranium–fluorine interaction. The structure is composed of isolated molecules, enabling a detailed examination of the U4+ (f2) ion. Characterization of single-crystals by X-ray diffraction, absorption spectroscopy, and magnetic analysis up to 45 T is combined with extensive theoretical treatment by CASSCF. The influence of different active spaces and representations of the structure is examined in the context of the experimental evidence. The Interacting Quantum Atoms method (IQA) is used to examine the nature of the U–F bond, concluding that there is a non-negligible degree of covalent character (9% of the total bond energy) in [UF8]4−. For the structural and theoretical reasons discussed herein, it is proposed that the structure of (NH4)4UF8 may be appropriately employed as a benchmark compound for future theoretical characterization of U(IV).Keywords
Funding Information
- National Science Foundation (DMR-1157490, DMR-1644779)
- U.S. Department of Energy (DE-SC0016568)
This publication has 73 references indexed in Scilit:
- The molten salt reactor (MSR) in generation IV: Overview and perspectivesProgress in Nuclear Energy, 2014
- Towards the thorium fuel cycle with molten salt fast reactorsAnnals of Nuclear Energy, 2014
- Fuel Salt for the Molten-Salt ReactorAtomic Energy, 2013
- Molten salt reactors: A new beginning for an old ideaNuclear Engineering and Design, 2010
- Thermal reactions of uranium metal, UO2, U3O8, UF4, and UO2F2 with NF3 to produce UF6Journal of Nuclear Materials, 2009
- Uranium and fluorine cycles in the nuclear industryJournal of Fluorine Chemistry, 2009
- Possible Configurations for the Thorium Molten Salt Reactor and Advantages of the Fast Nonmoderated VersionNuclear Science and Engineering, 2009
- Molten-Salt Reactors—History, Status, and PotentialNuclear Applications and Technology, 1970
- The First Isolation of PlutoniumJournal of the American Chemical Society, 1949
- The Vapor Pressure of Uranium HexafluorideThe Journal of Chemical Physics, 1948